Insights into Nitrate Reduction over Indium-Decorated Palladium Nanoparticle Catalysts

Guo, Sujin; Heck, Kimberly; Kasiraju, Sashank; Qian, Huifeng; Zhao, Zhun; Grabow, Lars C.; Miller, Jeffrey T.; Wong, Michael S.

doi:10.1021/acscatal.7b01371

Title: Insights into Nitrate Reduction over Indium-Decorated Palladium Nanoparticle Catalysts

Journal Article · Tue Nov 21 00:00:00 EST 2017 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.7b01371· OSTI ID:1485307

Guo, Sujin ^[1]; Heck, Kimberly ^[2]; Kasiraju, Sashank ^[3]; Qian, Huifeng ^[2]; Zhao, Zhun ^[2];

^[3]; Miller, Jeffrey T. ^[4];

^[5]

Rice Univ., Houston, TX (United States). Dept. of Civil and Environmental Engineering and Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment
Rice Univ., Houston, TX (United States). Dept. of Chemical and Biomolecular Engineering
Univ. of Houston, TX (United States). Dept. of Chemical and Biomolecular Engineering
Purdue Univ., West Lafayette, IN (United States). Chemical Engineering
Rice Univ., Houston, TX (United States). Dept. of Civil and Environmental Engineering, Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment, Dept. of Chemical and Biomolecular Engineering, Dept. of Chemistry, and Dept. of Materials Science and NanoEngineering

Nitrate (NO₃-) is an ubiquitous groundwater contaminant and is detrimental to human health. Bimetallic palladium-based catalysts have been found to be promising for treating nitrate (and nitrite, NO₂-) contaminated waters. Those containing indium (In) are unusually active, but the mechanistic explanation for catalyst performance remains largely unproven. Here, we report that In deposited on Pd nanoparticles (NPs) (“In-on-Pd NPs”) shows room-temperature nitrate catalytic reduction activity that varies with volcano-shape dependence on In surface coverage. The most active catalyst had an In surface coverage of 40%, with a pseudo-first order normalized rate constant of k_cat ~ 7.6 L g_{surface-metal}^-1 min^-1, whereas monometallic Pd NPs and In₂O₃ have nondetectible activity for nitrate reduction. X-ray absorption spectroscopy (XAS) results indicated that In is in oxidized form in the as-synthesized catalyst; it reduces to zerovalent metal in the presence of H₂ and reoxidizes following NO₃- contact. Selectivity in excess of 95% to nontoxic N₂ was validated for all the catalysts. Density functional theory (DFT) simulations indicate that submonolayer coverage amounts of metallic In provide strong binding sites for nitrate adsorption and they lower the activation barrier for the nitrate-to-nitrite reduction step. This improved understanding of the In active site expands the prospects of improved denitrification using metal-on-metal catalysts.

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0011983; AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1485307

Journal Information:: ACS Catalysis, Vol. 8, Issue 1; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 125 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
nitrate reduction
bimetallic catalyst
DFT
indium
palladium
core−shell

Title: Insights into Nitrate Reduction over Indium-Decorated Palladium Nanoparticle Catalysts

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